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Simulation of Liberattion and Transport of Radium from Uranium

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Simulation of Liberattion and Transport of Radium from Uranium Simulation of Liberation and Transport of Radium from Uranium Tailings Maria de Lurdes Dinis 1, António Fiúza 1Department of Mining Engineering, Research Center in Environment and Re- sources – CIGAR. Engineering Faculty of Oporto University. Rua Dr. Roberto Frias, s/n, 4200-465 Oporto, Portugal. [email protected];[email protected]. Abstract. The uranium tailings contain a large amount of radium, besides other radionuclides like uranium, thorium, polonium and lead. The transport and fate of radionuclides in groundwater are assumed to follow the theoretical approach rep- resented by the basic diffusion/dispersion – advection equation. Our algorithm uses the analytical solution for the one dimensional steady-state transport problem of a reactive substance with simultaneous retardation and radioactive decay. The final output is the radionuclides concentration in a hypothetical well location as function of the elapsed time. Introduction The environmental effects resulting from uranium mining activities are mainly de- rived from the wastes generated by the ore processing. Uranium mill tailings are the solid residues resulting from the leaching of the ores. The tailings possess, in their composition, hazardous radioactive and toxic by-products and are generally disposed in open air piles. Since only the first four isotopes in the uranium 238 decay series are extracted, all other member of the family remain in the tailings at their original activities. In addition, small residual amounts of uranium are left in the tailings, depending on the efficiency of the ex- traction process used. Although the activity in most uranium tailings is relatively low, some radiological hazard will last virtually forever because of the long half- life of the radionuclides involved. The uranium tailings disposal represents the highest potential source of envi- ronmental contamination for the great majority of uranium mining activities. Ap- proximately 70% of the original activity from uranium ore remains in the tailings and it is essentially due to the 230 Th and its descendents, in particular 226 Ra. The radionuclides in the tailings are more mobile and chemically reactive than in 2 Maria de Lurdes Dinis1, António Fiúza original ore. They are now potentially more able to enter in the environment by seepage, leaching and as dust, becoming a contamination source to the air, soil, superficial water and groundwater. Radium is often considered to be the most important radiotoxic decay product in the uranium decay series not only by its high radioactivity but because it also produces radon ( 222 Rn), an inert gas whose decay products can cause lung cancer. Airborne radon degrades into a series of short half-life decay products that are hazardous if inhaled. However, 210 Pb is also an important decay product, both be- cause of its radiotoxicity and because of the mobility of 210 Po, a subsequent daughter. Uranium mill tailings also contain potentially dangerous materials such as arse- nic and selenium. These toxic and other radioactive materials like radium and ura- nium may get into the human body mainly through the food chain if they are not properly disposed off. The transport of radionuclides from a site may occur by the infiltrated precipi- tation. As water percolates through the pores, some radionuclides are released from the pile where they are exposed, adsorbed to sediments or dissolved in water. This contaminated water may migrate downward to the subsoil and contaminate the groundwater. Once in the groundwater the radionuclides may become accessi- ble to humans or other forms of life when they reach a hypothetical well. The ra- dionuclides present in the water pumped from a well will represent a potential hazard to the nearby population resulting either from a possible ingestion or from its use for irrigation. This work proposes a two-direction model for simulating the radionuclides re- lease from a uranium tailings pile and its migration process through the soil to the groundwater. The final result is the radionuclide concentration in the groundwater as function of the elapsed time, at a defined distance from the pile, where is con- sidered to be located the well. Methods and Results The Release Mechanism The model is divided into three sub-models describing each one different proc- esses: (i) the release mechanism which accounts for the infiltrating water through the cover and the radionuclides leaching out from the contaminated material, (ii) the transport either in the vertical direction, downwards into the soil through the unsaturated zone until an aquifer is reached, either in the horizontal direction, through the saturated zone to the well, and finally (iii) the radionuclides concen- tration in the well water after the elapsed time. The algorithm may incorporate four zones with different properties for the ver- tical transport: the cover, the contaminated zone, the unsaturated zone and the Simulation of Liberation and Transport of Radium from Uranium Tailings 3 saturated zone. The source is considered homogenous, without taking in account the spatial distribution of the radionuclides activity, and is modelled as an infiltra- tion point where the vertical transport starts. A simple water balance concept is used to estimate the amount of infiltrating water into the soil which will leach the radionuclides from the contaminated ma- trix (IAEA 1992) . The annual infiltrating water rate can be estimated as a function of the cover failure. It may be necessary to consider both components: the intact portion and the failed portion. For the failed portion, the inflow rate will increase as a consequence of the cover cracking or erosion effects. The infiltrated water will leach some radionuclides adsorbed in soil being con- taminated after the contact with the waste material. A simplified model is adopted in our work considering a single-region flow transport where the water flow is as- sumed to be uniform through relatively homogeneous layers of soil profile (EPA 1996). The simplified model assumes an idealized steady-state and uniform leach- ing process to estimate the radionuclides concentration in the infiltrated water based on a chemical exchange process. The leaching model is characterized by a sorption-desorption process where the radionuclide concentration is estimated as a function of the equilibrium partioning between the solid material and the solution. The degree of sorption between the two phases is described by a distribution or partitioning coefficient, Kd. The fol- lowing equation is used to estimate the leachate concentration under equilibrium partitioning conditions (EPA 1996; Hung 2000): = [ ( θ + ρ )] C wt I t A D D K d (1) 3 From the above equation, it is known that leachate concentration, C wt (Bq/m ) is 3 determined by (1) its K d (cm /g) value, which decides the relative transport speed of the radionuclide to that of water in the pore space; (2) soil properties such as bulk density, ρ (g/cm 3), the volumetric water content, θ (dimensionless); and (3) the extent of contamination, which is described by the contaminated zone thick- 2 ness, D (m), area, A (m ) and the amount of radionuclide activity in the source, I t (Bq). Another important mechanism of release is uncontrolled seepage of contami- nated liquids contained in the tailings pile. Seepage may initially occur due to the tailings liquids associated with the solids when placed. However, in a longer term, seepage is provoked by water seeping into the tailings moving the radionuclides as water moves through and out of the tailings (IAEA 1992). The Radionuclides transport The Vertical Transport The radionuclides are considered to be mobilized sequentially in two directions: vertically downwards into the soil until it reaches an aquifer and then horizontally through the aquifer to a hypothetical well. 4 Maria de Lurdes Dinis1, António Fiúza The flow in the vertical direction is simulated for different degrees of saturation depending on the properties of the geologic strata involved. It is also assumed that there is retardation during the vertical transport. The retardation factor (Rv ) is the ratio of the average pore water velocity to the radionuclide transport velocity and is calculated assuming that adsorption-desorption process can be represented by a linear isotherm. Following the simplest mathematical approach derived from the Freudlich isotherm equation, the retardation factor can be estimated with the fol- lowing formula (EPA 1996; Hung 2000): ρK R =1+ d (2) v ε R s Concentrations of radionuclides in the well water are time-dependent and are function of two transport times – the breakthrough time (vertical transport time to reach the aquifer) and the rise time (horizontal transport time to reach the well). These parameters are combined to estimate the time necessary to transport verti- cally the radionuclides to the aquifer and also the water velocity in the vertical di- rection. The Horizontal Transport Among the great variety of hydrologic models available in the literature describ- ing the contaminants transport in groundwater, most of them fail in considering the process of radionuclide decay and its sorption and in this way these models are not adjusted for the exposure assessment purpose. Radionuclides transport and fate in groundwater follow the theoretical approach of the transport processes represented by the basic diffusion/dispersion-advection equation. The model uses the analytical solution for the one dimensional steady- state transport problem of a reactive substance with radioactive decay. The general equation describing the mass conservation law applied to a reactive solute can be represented by: ∂2C ∂C r ∂C D − V ± = (3) ∂x2 ∂x θ ∂t In this equation, D represents the molecular diffusion coefficient (L2.T-1), C represents the solute concentration (M.L-3), V represents the interstitial velocity (L.T -1), θ represents the moisture content (dimensionless) and the r represents the mass produced or consumed. The term ± r/ θ may have different forms depending on the kind of reactions involved.
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